<p>Dendrite growth represents one of the most&#xa0;significant challenges that impede the development of aqueous zinc-ion batteries. Herein, Gd<sup>3+</sup> ions are introduced into conventional electrolytes as a microlevelling agent to achieve dendrite-free zinc electrodeposition. Simulation and experimental results demonstrate that these Gd<sup>3+</sup> ions are preferentially adsorbed onto the zinc surface, which enables dendrite-free zinc anodes by activating the microlevelling effect during electrodeposition. In addition, the Gd<sup>3+</sup> additives effectively inhibit side reactions and facilitate the desolvation of [Zn(H<sub>2</sub>O)<sub>6</sub>]<sup>2+</sup>, leading to highly reversible zinc plating/stripping. Due to these improvements, the zinc anode demonstrates&#xa0;a significantly prolonged cycle life of&#xa0;2100 h and achieves an exceptional average Coulombic efficiency of 99.72% over 1400 cycles. More importantly, the Zn//NH<sub>4</sub>V<sub>4</sub>O<sub>10</sub> full cell shows a high capacity retention rate of 85.6% after 1000 cycles. This work not only&#xa0;broadens the &#xa0;application of metallic cations in battery electrolytes&#xa0;but also&#xa0;provides fundamental insights into their working mechanisms.</p>

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Cationic Adsorption-Induced Microlevelling Effect: A Pathway to Dendrite-Free Zinc Anodes

  • Long Jiang,
  • Yiqing Ding,
  • Le Li,
  • Yan Tang,
  • Peng Zhou,
  • Bingan Lu,
  • Siyu Tian,
  • Jiang Zhou

摘要

Dendrite growth represents one of the most significant challenges that impede the development of aqueous zinc-ion batteries. Herein, Gd3+ ions are introduced into conventional electrolytes as a microlevelling agent to achieve dendrite-free zinc electrodeposition. Simulation and experimental results demonstrate that these Gd3+ ions are preferentially adsorbed onto the zinc surface, which enables dendrite-free zinc anodes by activating the microlevelling effect during electrodeposition. In addition, the Gd3+ additives effectively inhibit side reactions and facilitate the desolvation of [Zn(H2O)6]2+, leading to highly reversible zinc plating/stripping. Due to these improvements, the zinc anode demonstrates a significantly prolonged cycle life of 2100 h and achieves an exceptional average Coulombic efficiency of 99.72% over 1400 cycles. More importantly, the Zn//NH4V4O10 full cell shows a high capacity retention rate of 85.6% after 1000 cycles. This work not only broadens the  application of metallic cations in battery electrolytes but also provides fundamental insights into their working mechanisms.